Pulse‐field evaporation of III–V compound semiconductors was investigated employing our high‐performance time‐of‐flight atom probe, which accommodates the demand for precise knowledge of both mass (focusing type) and energy deficits (straight type) of field‐evaporated ion species. We show that laser‐pulse mode can yield correct compositions only if an appropriate dc holding field range is used, which is 0.35 to 0.65 for the GaAs presently studied.